Production of nitrogenous compounds.



PAUL RAISE I-IERSHMAN, CHICAGQ, ILLINOIS, ASSIGINQR T ABMG'D'R FERTILIZER WORKS, OF CHICAGO, ILLINOIS, A COREORATXON OF NEW JERSEY.

IRODUGTION OF 'HII'ROGENOUS GGMZPQUIQ'ES.

115%,? X it Specification of Iiio Drawing. Application filed November To all whom concern Be it known that I, PAUL RALPH Hunsu- MAN, a citizen of AustriwHungary, residing at Chicago, in the county of Cook and State of Illinois, have ii'ivcnted certainnew anduseful Improvements in the Production of Nitrogenous Compounds, of which the following is a specification,

One of the leading purposes of the present invention resides in the provision of a novel and improved method or process of producing nitrogenous compounds in an emcient and economical manner, such, for example, as the production of aluminum nitrid from aluminum oxid.

Complete nitrification of the aluminum can be obtained when a mass orgmixture of aluminum compounds, such as an oxidfaixd; carbon in any suitable form, is heated'ata temperature of approximately 1500S centigrade, in the presence of carbon monoxid, or carbon monoxid and hydrogen, commercially known as Water gas, under which circumstances, the aluminum oxid .is seemingly changed into a carbid compound containing less carbon than corresponds to the formula A1 6,, and then the resulting com; pounds are converted into nitride by heating at approximately 1500 to 1600 centigrade, in a current of nitrogen, or a mixture or nitrogen and a reducing gas, such as hydro;-

rgen, V

The heating of the aluminum compound as described has a tendency tofac-ili-tate the, subsequent production. of nitrids by carry-1' ing out the process, so to speak, in two stages; in the first stage there are formed compounds consisting largely of aluminum and carbon, with apparently less carbon than would be represented in the formula, ALC and there ispossibly a formation of metallic aluminum particles, aseis evidenced by the fact that the mixture when treated with sodium hydroxid solution before it is subjected to the subsequent treatment with nitrogen evolves hydrogen. It is, however, possible that the reasonthat the compounds thus formed are more easily subjected to combination with nitrogen lie partly in the fact that the original compound of the formula Al O ispartly reduced to a 001m pound of the formula, A10, such as described by Ninkler. The reactions maybe further facilitated and aided by the employ ment of a carrying; agent capable of combin Letters en Patented dune 2ft, 1e16,

8,1915. Seria.1lbl'o.6t),262.

ing with nitrogen, and, preferably, one which may combine with nitrogen in more than one proportion A; variation of the process consists.- in heeting theresulting mass before it is sub ected to the action of nitrogen, for a short time, in a current of carbon dioxid. it appears that through thisheating the reduction of the oxygen-containing, aluminum compounds is facilitated, and that they are deprived =of an additional part ofthe oxygen which they contain. The carbon dioxid I can be derived easily, for instance, from smoke or-fiue gas, provided it contains no nitrogen, such as is formed when. water gas is used, and deprived of the H 0 vapor formed by the combustion, by cooling in any preferred manner.

A desirable way of carrying out the proceSs'is substantially as follows: A. powdered mixture or mass in about the proportion of one molecule of aluminum oxid to at least six atoms of carbon, and, it-preterrcd, from shelf-to five per cent. of the Weight of the mixtureot a. carrying" agent, for instance, titanium or calcium compounds, or similar "compounds reducible by carbon, is heated at a temperature of approximately 15043 centi grade in a current of water gas, which sults in a reduction of the aluminum :id to a product containing more or less carbon. in chemical combination with aluminum. e hydrogen of the water gas assists in be mation of the compounds mcnti :diovc and the combined eiifcrt of monoxid and hydrogen is strong, 211 that of the components used scparat y o" ccssion in the same time period, l more, it is more economical to carry out the process in this way than by attempti use either of the two ingredients separu. 1

This product is then heated in a. current of carbon dioxid to effect further reduction either to sub-carbide: or metal, which re duction aids the subsequent union nitrogen. Then these carbide are changed into nitrids by heating at a temperature of approximately 1590 to MOO centigrade, in a current, of nitrogen or a mixture of; nitrogen and a reducing; gas, such, for ex ample, as hydrogen.

The employment of the aids and facilitates the re: on, that is, the union of the nitro en wi i-the aluminum, the carrying'e'geni ingredient apparently carrying ageht u o r with forming an unstable compound with the nitrogen, and in case a reducing gas is employed, the combination of the carryingagent-With the nitrogen of a higher proportion is reduced by the hydrogen of the gas, facilitating the production of aluminum nitrid.

This process is susceptible of variations with respect to the ingredients employed, the proportion of parts used, and the temperatures maintained, and it is, therefore, to be understood that the invention is not limited and restricted to the precise and exact features of the methods set forth. For example, the carbon monoxid without hydrogen might be used and the step employing the carbon dioxid may be omitted, but I have found that the practice of the process as set forth is a preferred Way of utilizing the invention.

1 claim:

1, The method of producing nitrogenous compounds of aluminum which consists in heating a mixture of aluminum oxid and carbon-in carbon monoxid practically free from nitrogen, and then in a gas containing nitrogen, substantially as described.

The method of producing nitrogenous compounds of aluminum which consists in heating a mixture of aluminum oxid and carbon in a gas consisting principally of carbon monoxid and hydrogen, and then in a containing nitrogen, substantially as described.

3. The method of producing nitrogenous compounds of aluminum which consists in heating a mixture of aluminum oxid, carbon, and a carrying agent capable of combining with nitrogen. in carbon monoxid practically tree from nitrogen, and then in a gas containing nitrogen, substantially as described.

-l'. The method of producing nitrogenous compoumls of aluminum which consists in heating a mixture of aluminum oxid, carbon. and a carrying agent capable of combining with nitrogen, in a gas consisting i'n-incipally of carbon uionoxid and h \'drogen, and then in a "a containing nitrogen,- substantially as described.

5. The method of producing nitrogenous compounds of aluminnm \\lll(fl consists in heating a mixture of aluminum oXid. carbon, and a cariyii'ig agent capable of com bining with liltl' ),L' 'lll in more than one proportion. in carbon mouoxid, and'then in a gas containing nitrogen and hydrogen, the combination of the carryiag agent and nitrogen oi a higher proportion being reduced'by the hydrogen, slibstant-ially as described.

:"i. The method or producing nitrogenous hich consists in heating a mix ml at term! to be 4 u I combined oxid, then in carbon dioxid, and then in a gas containing nitrogen, substantially as described.

7. The method of producing. nitrogenous compounds which consists in heating a mixture of aluminum oxid and carbon, in car,- bon monoxicl, then in carbon dioxid, and then in a gas containing nitrogen, substantially as described.

8. The method of producing nitrogeous compounds which consists in heating a nixture of aluminum oxid and carbon, in' a gas consisting principally of carbon monoxid and hydrogen, then in carbon dioxid, and then in a gas containing nitrogen, substantially as described.

9. The method of producingnitrogenous compounds which consists of heating-a mixture of the material to be combined with the nitrogen, carbon, and a carrying agent capable of combining with nitrogen, in carbon monoxid, then in-carbon dioxid, and then in a gas containing nitrogen, substantially as described.

10. The method of producing nitrogenous compounds which consists in heating a mixture of the material to be combined with the nitrogen, carbon, and a. carrying agent capable of combihing with the nitrogen, in a gas consisting princi rally of carbon monoxid and hydrogen, then in carbon dioxid, and then in a gas containing nitrogen, substantially as described.

11. The method of producing nitrogenous compounds of 'aluminum which consists in heating a mixture of aluminum oxid, carbon, and a carrying agentcapable of combining with nitrogen, in carbon monoxid, then in czv'bon dioxid, and then in-a gas containing nitrogen, substantially as described.

12. The method of producing nitrogenous compounds of aluminum which consists in heating a mixture of aluminum o.\ id, carbon, and a carrying agent capable of com bining with nitrogen, in a gas consisting;

principally of carbon monoxid and hydrogen, then in carbon dioxid, and then in a gas containing nitrogen, substantially as described.

13. The method of producing nitrogenous compounds which consists in heating a mixture otaluininum oxid, carbon, and a carry in, agent capable of combining with nitrogen in more than one proportion, in carbon monoxid, then in carbon dioxid, and then in a gas containing nitrogen, substantially as described.

14'. The method of producing nitrogenous compounds which consists in heating a. mixture of aluminum oxid, carbon, and a carrying agent capable of combining with nitrogen in more than one proportion, in a gas consisting principally oi carbon monoxid and hydrogen, then in carbon dioxid, and

"1500" centigrade, and

1500 centigrade, and than subjecting it to the action of nitrogen, substantially as de- 16. The method producing nitrogenous compounds ot aluminum which consists in heating a mixture in the proportion of one. molecule of aluminum mud to not less than slX atoms of carbon, in a current of gas consisting principally of carbon monoxid and hydrogen at a temperature of approximately then sub ectmg it to the action of nitrogen, substantially as de-' scribed.

11'. The method of produc ng nitrogenous compounds oi aluminum which consists in heating a mixture in approximately the proportion of one molecule of aluminum oxid to'not less than six atoms of carbon and con taining a carrying-agent capable of combincompounds of ing with nitrogen, in a current of carbon monoxid at a temperatureoi' approximately 1500" centigrade and then subgecting it to the action. of nitrogen,substantially as described.

18. T he method of producing nitrogenous compounds of aluminum which consists in heating a mixture of approximately the proportion of one molecule oi aluminum oxid to not less than six atoms of carbon, and containing a carrying agent capable of combining with nitrogen ina current of gas consisting principally of carbon monoxid and hydrogen, at a temperature of approximately il500 centigrade, and then subjecting it to the action of nitrogen,substantially as described.

19. The method of producing nitrogenous heating a mixture in approximately the pro nortion of one molecule of aluminum oxid to not less than atoms of carbon, and containing a carrying agent capable ott'orming an unstable conipoinii with nitrogen, in a current of gas consisting principally of carbon monoxid at a temperature oi? approximately 156% centigrade, and then subject aluminum which consists incarbon dioxid, and then to a gas containing nitrogen, substantially as described 21. The method of producing nitrogenous compounds of aluniinum'which consists in heating a mixture in approximately the proportion of one molecule of aluminum oxid to not less than six atoms'of carbon, and containinga carrying agent capable of combining with nitrogen in more than one proportion, in a current of carbon monoxid at a temperature of approximately 1500 centigrade, and then in a gas containing nitrogen, substantially as described.

, 22. The method of producin nitrogenous compounds of aluminum Whic consists in heating a mixture in approximately the proportion of one molecule of aluminum oxid to not less than six atoms of carbon, and containing a carrying agent capable of combining with nitrogen in more than one proporticn, in a current of gas consisting principally of carbon monoxid and hydrogen at a temperature ofapproximately 1:200" centigrade, and then in a gas containing nitrogen, substantially as described.

.23. The method of producing nitrogenous compounds of aluminum, which consists in heating a mixture in approximately the proportion of one molecule of aluminum oxid to not less than six atoms of carbon, and containing a carrying agent capable of combining with nitrogen in more than one proportion, in a current of gas consisting principally of carbon nionoxid and hydrogen, at a temperature of approximately 100 centigrade, then in carbon dioxid, anc then m a gas containing nitrogen, substantially as described. v a

- PAUL RALPH nnnsnMAN. 

